Highly Efficient Dual-Polar Electrochemiluminescence from Au25 Nanoclusters: The Next Generation of Multibiomarker Detection in a Single Step

Abstract

For the first time, simultaneous cathodic and anodic electrochemiluminescence (ECL) emissions of bull serum albumin stabilized Au25 nanoclusters (Au25 NCs) as highly efficient bipolar ECL probes were constructed for the single-step and synchronous determination of carcinoembryonic antigen (CEA) and mucin 1 (MUC1) based on different coreactant and coreaction accelerators. Under the potential cathodic scanning, TiO2 nanosheets (TiO2 NSs) as cathodic coreaction accelerators could catalyze the reduction of coreactant dissolved O2 for promoting cathodic ECL emission of Au25 NCs, while, under the potential anodic scanning, Cu2O@Cu nanoparticles (Cu2O@Cu NPs) as anodic coreaction accelerators could stimulate the oxidation of coreactant N,N-diethylethylenediamine (DEDA) for enhancing anodic ECL emission of Au25 NCs. Thus, the proposed strategy easily solved one main technical challenge of cross reactions of dual-luminophors for dual-biomarker detection, resulting in great sensitivity and accuracy toward the detection of CEA down to 0.43 pg/mL and MUC1 down to 5.8 fg/mL. As a proof of concept, this work realized single-step and simultaneous detection of dual biomarkers, which initiates a new thought in realizing a new generation of dual-biomarker ECL detection beyond the traditional ones in sensing analysis and diagnostic sensing.